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@ARTICLE{Schleutker:838295,
author = {Schleutker, Marco and Bahner, Jochen and Tsai, Chih-Long
and Stolten, Detlef and Korte, Carsten},
title = {{O}n the interfacial charge transfer between solid and
liquid {L}i + electrolytes},
journal = {Physical chemistry, chemical physics},
volume = {19},
number = {39},
issn = {1463-9084},
address = {Cambridge},
publisher = {RSC Publ.},
reportid = {FZJ-2017-06938},
pages = {26596--26605},
year = {2017},
abstract = {The Li+ ion transfer between a solid and a liquid Li+
electrolyte has been investigated by DC polarisation
techniques. The current density i is measured as a function
of the electrochemical potential drop Δ[small mu, Greek,
tilde]Li+ at the interface, using a liquid electrolyte with
different Li+ concentrations. The subject of this
experimental study is the interface between the solid
electrolyte Ta-substituted lithium lanthanum zirconate
(Li6.6La3Zr1.6Ta0.4O12) and a liquid electrolyte consisting
of LiPF6 dissolved in ethylene carbonate/dimethyl carbonate
(1 : 1). The functional course of i vs. Δ[small mu,
Greek, tilde]Li+ can be described by a serial connection
between a constant ohmic resistance Rslei and a current
dependent thermally activated ion transfer process. For the
present solid–liquid electrolyte interface the areal
resistance Rslei of the surface layer is independent of the
Li+ concentration in the liquid electrolyte. At room
temperature a value of about 300 Ω cm2 is found. The
constant ohmic resistance Rslei can be attributed to a
surface layer on the solid electrolyte with a (relatively)
low conductivity (solid–liquid electrolyte interphase).
The low conducting surface layer is formed by degradation
reactions with the liquid electrolyte. Rslei is considerably
increased if a small amount (ppm) of water is added to the
liquid electrolyte. The thermally activated ionic transfer
process obeys a Butler–Volmer like behaviour, resulting in
an exchange current density i0 depending on the Li+
concentration in the liquid electrolyte by a power-law. At a
Li+ concentration of 1 mol l−1 a value of 53.1 μA cm−2
is found. A charge transfer coefficient α of ∼0.44 is
measured. The finding of a superposed constant ohmic
resistance due to a solid–liquid electrolyte interphase
and a current dependent thermally activated ion transfer
process is confirmed by the results of two former
experimental studies from the literature, performing AC
measurements/EIS.},
cin = {IEK-3},
ddc = {540},
cid = {I:(DE-Juel1)IEK-3-20101013},
pnm = {131 - Electrochemical Storage (POF3-131)},
pid = {G:(DE-HGF)POF3-131},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:28948987},
UT = {WOS:000412763700013},
doi = {10.1039/C7CP05213H},
url = {https://juser.fz-juelich.de/record/838295},
}